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Nanosecond time-resolved dual-comb absorption spectroscopy

Nature Photonics volume 18, pages 127–131 (2024)Cite this article

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Abstract

Frequency combs have revolutionized the field of optical spectroscopy, enabling researchers to probe molecular systems with a multitude of accurate and precise optical frequencies. Although there have been tremendous strides in direct frequency comb spectroscopy, these approaches have been unable to record high-resolution spectra on the nanosecond-timescale characteristic of many physiochemical processes. Here we demonstrate a new approach to achieve optical frequency comb generation in which a pair of electro-optic combs is produced in the near-infrared regime and subsequently transferred with high mutual coherence and efficiency into the mid-infrared regime within a single optical parametric oscillator. The high power, mutual coherence and agile repetition rates of these combs, as well as the large mid-infrared absorption of many molecular species, enable fully resolved spectral transitions to be recorded in timescales as short as 20 ns. We have applied this approach to study the rapid dynamics occurring within a supersonic pulsed jet; however, we note that this method is widely applicable to fields such as chemical and quantum physics, atmospheric chemistry, combustion science and biology.

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Fig. 1: Instrumental schematic of the OPO-based, mid-infrared dual-comb spectrometer employed to interrogate a supersonic pulsed jet.
Fig. 2: Mid-infrared optical frequency comb interferograms and spectra.
Fig. 3: Measured change in the CO2 integrated absorption during the pulsed jet.
Fig. 4: Observed CO2 P26e transition integrated absorption during the falling edge of the pulsed jet for a range of chamber pressures.
Fig. 5: Observed CH4 transition integrated absorption change.

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Data availability

All data and supporting materials are available through the National Institute of Standards and Technology at https://doi.org/10.18434/mds2-3091.

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Acknowledgements

We thank P. Hamlington, K. Souders and J. T. Hodges for helpful discussions. We also acknowledge D. Foote for his many contributions. Certain equipment, instruments, software or materials are identified in this paper to adequately specify the experimental procedure. Such identification is not intended to imply recommendation or endorsement of any product or service by National Institute of Standards and Technology, nor is it intended to imply that the materials or equipment identified are necessarily the best available for the purpose. This material is based in part on work supported by the Air Force Office of Scientific Research under award nos. FA9550-20-1-0328 (C.M., G.C.M., A.F. and G.B.R.) and FA8650-20-2-2418 (C.M., G.C.M., A.F. and G.B.R.).

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Authors and Affiliations

  1. National Institute of Standards and Technology, Gaithersburg, MD, USA

    David A. Long

  2. TOPTICA Photonics, Pittsford, NY, USA

    Matthew J. Cich & Adam T. Heiniger

  3. Precision Laser Diagnostics Laboratory, University of Colorado, Boulder, CO, USA

    Carl Mathurin, Garrett C. Mathews, Augustine Frymire & Gregory B. Rieker

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Contributions

This work was conceptualized by D.A.L., M.J.C., A.T.H. and G.B.R. as well as investigated by D.A.L., M.J.C., C.M., G.C.M., A.F. and G.B.R. The funding was acquired by D.A.L., M.J.C., A.T.H. and G.B.R. The original draft of the manuscript was prepared by D.A.L., C.M. and A.T.H., with all authors assisting with reviewing and editing.

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Correspondence to David A. Long.

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Competing interests

M.J.C. and A.T.H. are/were employed by TOPTICA Photonics. TOPTICA Photonics has submitted a patent related to this work and manufactured a portion of the equipment used in this work. The remaining authors declare no competing interests.

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Supplementary Sections 1–3 and Fig. 1.

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Long, D.A., Cich, M.J., Mathurin, C. et al. Nanosecond time-resolved dual-comb absorption spectroscopy. Nat. Photon. 18, 127–131 (2024). https://doi.org/10.1038/s41566-023-01316-8

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